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1.
ACS Nano ; 14(1): 1196-1206, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31904217

RESUMO

Hybrid light-matter states-polaritons-have attracted considerable scientific interest recently, motivated by their potential for development of nonlinear and quantum optical schemes. To realize such states, monolayer transition metal dichalcogenides (TMDCs) have been widely employed as excitonic materials. In addition to neutral excitons, TMDCs host charged excitons, which enables active tuning of hybrid light-matter states by electrical means. Although several reports demonstrated charged exciton-polaritons in various systems, the full-range interaction control attainable at room temperature has not been realized. Here, we demonstrate electrically tunable charged exciton-plasmon polaritons in a hybrid tungsten disulfide (WS2) monolayer-plasmonic nanoantenna system. We show that electrical gating of monolayer WS2 allows tuning the oscillator strengths of neutral and charged excitons not only at cryogenic but also at room temperature, both at vacuum and atmospheric pressure. Such electrical control enables a full-range tunable switching from strong neutral exciton-plasmon coupling to strong charged exciton-plasmon coupling. Our experimental findings allow discussing beneficial and limiting factors of charged exciton-plasmon polaritons, as well as offer routes toward realization of charged polaritonic devices at ambient conditions.

2.
ACS Nano ; 14(1): 28-117, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31478375

RESUMO

The discovery of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and analytical techniques. Significant experimental and theoretical effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technology, but additional efforts are still needed before it can be routinely used analytically and in commercial products. In this Review, prominent authors from around the world joined together to summarize the state of the art in understanding and using SERS and to predict what can be expected in the near future in terms of research, applications, and technological development. This Review is dedicated to SERS pioneer and our coauthor, the late Prof. Richard Van Duyne, whom we lost during the preparation of this article.

3.
Nano Lett ; 19(11): 8171-8181, 2019 11 13.
Artigo em Inglês | MEDLINE | ID: mdl-31639311

RESUMO

Polaritons are compositional light-matter quasiparticles that have enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Recently, plasmon-exciton polaritons (plexcitons) have been realized in hybrid material systems composed of transition metal dichalcogenide (TMDC) materials and metal nanoparticles, expanding polaritonic concepts to room temperature and nanoscale systems that also benefit from the exotic properties of TMDC materials. Despite the enormous progress in understanding TMDC-based plexcitons using optical-based methods, experimental evidence of plexcitons formation has remained indirect and mapping their nanometer-scale characteristics has remained an open challenge. Here, we demonstrate that plexcitons generated by a hybrid system composed of an individual silver nanoparticle and a few-layer WS2 flake can be spectroscopically mapped with nanometer spatial resolution using electron energy loss spectroscopy in a scanning transmission electron microscope. Experimental anticrossing measurements using the absorption-dominated extinction signal provide the ultimate evidence for plexciton hybridization in the strong coupling regime. Spatially resolved EELS maps reveal the existence of unexpected nanoscale variations in the deep-subwavelength nature of plexcitons generated by this system. These findings pioneer new possibilities for in-depth studies of the local atomic structure dependence of polariton-related phenomena in TMDC hybrid material systems with nanometer spatial resolution.

4.
Nat Commun ; 10(1): 3336, 2019 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-31350397

RESUMO

Strong light-matter interactions in both the single-emitter and collective strong coupling regimes attract significant attention due to emerging applications in quantum and nonlinear optics as well as opportunities for modifying material-related properties. Exploration of these phenomena is theoretically demanding, as polaritons exist at the intersection between quantum optics, solid state physics, and quantum chemistry. Fortunately, nanoscale polaritons can be realized in small plasmon-molecule systems, enabling treatment with ab initio methods. Here, we show that time-dependent density-functional theory calculations access the physics of nanoscale plasmon-molecule hybrids and predict vacuum Rabi splitting. By considering a system comprising a few-hundred-atom aluminum nanoparticle interacting with benzene molecules, we show that cavity quantum electrodynamics holds down to resonators of a few cubic nanometers in size, yielding a single-molecule coupling strength exceeding 200 meV due to a massive vacuum field of 4.5 V · nm-1. In a broader perspective, ab initio methods enable parameter-free in-depth studies of polaritonic systems for emerging applications.

5.
Nat Nanotechnol ; 14(7): 679-683, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31061517

RESUMO

Monolayer transition metal dichalcogenides (TMDCs) have recently been proposed as an excitonic platform for advanced optical and electronic functionalities1-3. However, in spite of intense research efforts, it has not been widely appreciated that TMDCs also possess a high refractive index4,5. This characteristic opens up the possibility to utilize them to construct resonant nanoantennas based on subwavelength geometrical modes6,7. Here, we show that nanodisks, fabricated from exfoliated multilayer WS2, support distinct Mie resonances and anapole states8 that can be tuned in wavelength over the visible and near-infrared range by varying the nanodisk size and aspect ratio. As a proof of concept, we demonstrate a novel regime of light-matter interaction-anapole-exciton polaritons-which we realize within a single WS2 nanodisk. We argue that the TMDC material anisotropy and the presence of excitons enrich traditional nanophotonics approaches based on conventional high-index materials and/or plasmonics.

6.
Nano Lett ; 19(1): 189-196, 2019 01 09.
Artigo em Inglês | MEDLINE | ID: mdl-30500202

RESUMO

Polaritons are compositional light-matter quasiparticles that arise as a result of strong coupling between the vacuum field of a resonant optical cavity and electronic excitations in quantum emitters. Reaching such a regime is often hard, as it requires materials possessing high oscillator strengths to interact with the relevant optical mode. Two-dimensional transition metal dichalcogenides (TMDCs) have recently emerged as promising candidates for realization of strong coupling regime at room temperature. However, these materials typically provide coupling strengths in the range of 10-40 meV, which may be insufficient for reaching strong coupling with low quality factor resonators. Here, we demonstrate a universal scheme that allows a straightforward realization of strong coupling with 2D materials and beyond. By intermixing plasmonic excitations in nanoparticle arrays with excitons in a WS2 monolayer inside a resonant metallic microcavity, we fabricate a hierarchical system with the collective microcavity-plasmon-exciton Rabi splitting exceeding ∼500 meV at room temperature. Photoluminescence measurements of the coupled systems show dominant emission from the lower polariton branch, indicating the participation of excitons in the coupling process. Strong coupling has been recently suggested to affect numerous optical- and material-related properties including chemical reactivity, exciton transport, and optical nonlinearities. With the universal scheme presented here, strong coupling across a wide spectral range is within easy reach and therefore exploration of these exciting phenomena can be further pursued in a much broader class of materials.

7.
Nano Lett ; 18(9): 5522-5529, 2018 09 12.
Artigo em Inglês | MEDLINE | ID: mdl-30071168

RESUMO

Halide perovskites are known to support excitons at room temperatures with high quantum yield of luminescence that make them attractive for all-dielectric resonant nanophotonics and meta-optics. Here we report the observation of broadly tunable Fano resonances in halide perovskite nanoparticles originating from the coupling of excitons to the Mie resonances excited in the nanoparticles. Signatures of the photon-exciton (" hybrid") Fano resonances are observed in dark-field spectra of isolated nanoparticles, and also in the extinction spectra of aperiodic lattices of such nanoparticles. In the latter case, chemical tunability of the exciton resonance allows reversible tuning of the Fano resonance across the 100 nm bandwidth in the visible frequency range, providing a novel approach to control optical properties of perovskite nanostructures. The proposed method of chemical tuning paves the way to an efficient control of emission properties of on-chip-integrated light-emitting nanoantennas.

8.
Nano Lett ; 18(9): 5938-5945, 2018 09 12.
Artigo em Inglês | MEDLINE | ID: mdl-30081635

RESUMO

Monolayer transition-metal dichalcogenides (TMDCs) have attracted a lot of research attention recently, motivated by their remarkable optical properties and potential for strong light-matter interactions. Realization of strong plasmon-exciton coupling is especially desirable in this context because it holds promise for the enabling of room-temperature quantum and nonlinear optical applications. These efforts naturally require investigations at a single-nanoantenna level, which, in turn, should possess a compact optical mode interacting with a small amount of excitonic material. However, standard plasmonic nanoantenna designs such as nanoparticle dimers or particle-on-film suffer from misalignment of the local electric field in the gap with the in-plane transition dipole moment of monolayer TMDCs. Here, we circumvent this problem by utilizing gold bi-pyramids (BPs) as very efficient plasmonic nanoantennas. We demonstrate strong coupling between individual BPs and tungsten diselenide (WSe2) monolayers at room temperature. We further study the coupling between multilayers of WSe2 and BPs to elucidate the effect of the number of layers on the coupling strength. Importantly, BPs adopt a reduced-symmetry configuration when deposited on WSe2, such that only one sharp antenna tip efficiently interacts with excitons. Despite the small interaction area, we manage to achieve strong coupling, with Rabi splitting exceeding ∼100 meV. Our results suggest a feasible way toward realizing plasmon-exciton polaritons involving nanoscopic areas of TMDCs, thus pointing toward quantum and nonlinear optics applications at ambient conditions.

9.
Sci Adv ; 4(7): eaas9552, 2018 07.
Artigo em Inglês | MEDLINE | ID: mdl-29984306

RESUMO

Intermixed light-matter quasi-particles-polaritons-have unique optical properties owing to their compositional nature. These intriguing hybrid states have been extensively studied over the past decades in a wide range of realizations aiming at both basic science and emerging applications. However, recently, it has been demonstrated that not only optical but also material-related properties, such as chemical reactivity and charge transport, may be significantly altered in the strong coupling regime of light-matter interactions. We show that a nanoscale system, composed of a plasmonic nanoprism strongly coupled to excitons in a J-aggregated form of organic chromophores, experiences modified excited-state dynamics and, therefore, modified photochemical reactivity. Our experimental results reveal that photobleaching, one of the most fundamental photochemical reactions, can be effectively controlled and suppressed by the degree of plasmon-exciton coupling and detuning. In particular, we observe a 100-fold stabilization of organic dyes for the red-detuned nanoparticles. Our findings contribute to understanding of photochemical properties in the strong coupling regime and may find important implications for the performance and improved stability of optical devices incorporating organic dyes.

10.
Nano Lett ; 18(3): 1777-1785, 2018 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-29369640

RESUMO

Formation of dressed light-matter states in optical structures, manifested as Rabi splitting of the eigen energies of a coupled system, is one of the key effects in quantum optics. In pursuing this regime with semiconductors, light is usually made to interact with excitons, electrically neutral quasiparticles of semiconductors; meanwhile interactions with charged three-particle states, trions, have received little attention. Here, we report on strong interaction between localized surface plasmons in silver nanoprisms and excitons and trions in monolayer tungsten disulfide (WS2). We show that the plasmon-exciton interactions in this system can be efficiently tuned by controlling the charged versus neutral exciton contribution to the coupling process. In particular, we show that a stable trion state emerges and couples efficiently to the plasmon resonance at low temperature by forming three bright intermixed plasmon-exciton-trion polariton states. Our findings open up a possibility to exploit electrically charged polaritons at the single nanoparticle level.

11.
Nano Lett ; 17(1): 551-558, 2017 01 11.
Artigo em Inglês | MEDLINE | ID: mdl-28005384

RESUMO

Plasmon-exciton interactions are important for many prominent spectroscopic applications such as surface-enhanced Raman scattering, plasmon-mediated fluorescence, nanoscale lasing, and strong coupling. The case of strong coupling is analogous to quantum optical effects studied in solid state and atomic systems previously. In plasmonics, similar observations have been almost exclusively made in elastic scattering experiments; however, the interpretation of these experiments is often cumbersome. Here, we demonstrate mode splitting not only in scattering, but also in photoluminescence of individual hybrid nanosystems, which manifests a direct proof of strong coupling in plasmon-exciton nanoparticles. We achieved these results due to saturation of the mode volume with molecular J-aggregates, which resulted in splitting up to 400 meV, that is, ∼20% of the resonance energy. We analyzed the correlation between scattering and photoluminescence and found that splitting in photoluminescence is considerably less than that in scattering. Moreover, we found that splitting in both photoluminescence and scattering signals increased upon cooling to cryogenic temperatures. These findings improve our understanding of strong coupling phenomena in plasmonics.


Assuntos
Corantes Fluorescentes/química , Nanopartículas Metálicas/química , Prata/química , Ressonância de Plasmônio de Superfície , Luminescência , Microscopia Eletrônica de Varredura , Fenômenos Físicos
12.
Opt Express ; 24(18): 20373-81, 2016 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-27607644

RESUMO

We investigate the role of material loss and mode volume of plasmonic nanostructures on strong plasmon-exciton coupling. We find that the field enhancement, and therefore loss, is not important for the magnitude of the Rabi splitting as such, but instead it is determined by the mode volume. Nevertheless, for reaching true strong coupling condition, that is, coupling greater than any dissipation, it is important to compromise losses. We also show that using such popular geometries as a dimer of two spheres or bow-tie nanoantennas, does not allow compressing the mode volume much in comparison to a single nanoparticle case, except for very narrow gaps, but rather it allows for efficient extraction of the mode out of the metal thus making it more accessible for excitons to interact with. Even more efficient mode extraction is achieved when high refractive index dielectric is placed in the gap. Our findings may find practical use for quantum plasmonics applications.

13.
Nanoscale ; 7(21): 9405-10, 2015 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-25952612

RESUMO

Nanoplasmonic substrates with optimized field-enhancement properties are a key component in the continued development of surface-enhanced Raman scattering (SERS) molecular analysis but are challenging to produce inexpensively in large scale. We used a facile and cost-effective bottom-up technique, colloidal hole-mask lithography, to produce macroscopic dimer-on-mirror gold nanostructures. The optimized structures exhibit excellent SERS performance, as exemplified by detection of 2.5 and 50 attograms of BPE, a common SERS probe, using Raman microscopy and a simple handheld device, respectively. The corresponding Raman enhancement factor is of the order 10(11), which compares favourably to previously reported record performance values.

14.
Phys Rev Lett ; 114(15): 157401, 2015 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-25933338

RESUMO

Realizing strong light-matter interactions between individual two-level systems and resonating cavities in atomic and solid state systems opens up possibilities to study optical nonlinearities on a single-photon level, which can be useful for future quantum information processing networks. However, these efforts have been hampered by unfavorable experimental conditions, such as cryogenic temperatures and ultrahigh vacuum, required to study such systems and phenomena. Although several attempts to realize strong light-matter interactions at room temperature using plasmon resonances have been made, successful realizations on the single-nanoparticle level are still lacking. Here, we demonstrate the strong coupling between plasmons confined within a single silver nanoprism and excitons in molecular J aggregates at ambient conditions. Our findings show that deep subwavelength mode volumes V together with quality factors Q that are reasonably high for plasmonic nanostructures result in a strong-coupling figure of merit-Q/sqrt[V] as high as ∼6×10^{3} µm^{-3/2}, a value comparable to state-of-the-art photonic crystal and microring resonator cavities. This suggests that plasmonic nanocavities, and specifically silver nanoprisms, can be used for room temperature quantum optics.

15.
ACS Nano ; 8(9): 9286-94, 2014 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-25182843

RESUMO

Quasicrystals are structures that possess long-range order without being periodic. We investigate the unique characteristics of a photonic quasicrystal that consists of plasmonic Ag nanodisks arranged in a Penrose pattern. The quasicrystal scatters light in a complex but spectacular diffraction pattern that can be directly imaged in the back focal plane of an optical microscope, allowing us to assess the excitation efficiency of the various diffraction modes. Furthermore, surface plasmon polaritons can be launched almost isotropically through near-field grating coupling when the quasicrystal is positioned close to a homogeneous silver surface. We characterize the dispersion relation of the different excited plasmon modes by reflection measurements and simulations. It is demonstrated that the quasicrystal in-coupling efficiency is strongly enhanced compared to a nanoparticle array with the same particle density but only short-range lateral order. We envision that the system can be useful for a number of advanced light harvesting and optoelectronic applications.

16.
Sci Rep ; 3: 3074, 2013 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-24166360

RESUMO

We studied scattering and extinction of individual silver nanorods coupled to the J-aggregate form of the cyanine dye TDBC as a function of plasmon--exciton detuning. The measured single particle spectra exhibited a strongly suppressed scattering and extinction rate at wavelengths corresponding to the J-aggregate absorption band, signaling strong interaction between the localized surface plasmon of the metal core and the exciton of the surrounding molecular shell. In the context of strong coupling theory, the observed "transparency dips" correspond to an average vacuum Rabi splitting of the order of 100 meV, which approaches the plasmon dephasing rate and, thereby, the strong coupling limit for the smallest investigated particles. These findings could pave the way towards ultra-strong light-matter interaction on the nanoscale and active plasmonic devices operating at room temperature.

17.
Opt Express ; 20(10): 10816-26, 2012 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-22565705

RESUMO

We present a method for calculating the differential scattering cross sections from nanostructures close to an interface separating two semi-infinitive dielectric media. The method combines a fast finite element software (Comsol multiphysics), used for calculations of the fields around and inside the structure, and the Green's functions method, which is used to find the far field distribution from the calculated total fields inside the nanostructure. We apply the method to calculations of scattering spectra from silver nanowires supported by an air-glass interface, a system that is of high current interest in relation to various nanophotonics applications. The results are analyzed in relation to analytical models and compared to experimentally measured spectra, to which we find a good agreement.


Assuntos
Nanoestruturas/química , Nanofios , Ar , Algoritmos , Eletroquímica/métodos , Análise de Elementos Finitos , Vidro , Cinética , Luz , Modelos Estatísticos , Nanotecnologia , Espalhamento de Radiação , Prata/química , Software , Ressonância de Plasmônio de Superfície/métodos
18.
Nano Lett ; 12(5): 2464-9, 2012 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-22449167

RESUMO

Nanoplasmonic sensing is typically based on quantification of changes in optical extinction or scattering spectra. Here we explore the possibility of facile self-referenced hydrogen sensing based on angle-resolved spectroscopy. We found that heterodimers built from closely spaced gold and palladium nanodisks exhibit pronounced directional scattering, that is, for particular wavelengths, much more light is scattered toward the Au than toward the Pd particle in a dimer. The effect is due to optical phase shifts associated with the material asymmetry and therefore highly sensitive to changes in the permittivity of Pd induced by hydrogen loading. In a wider perspective, the results suggest that directional scattering from bimetallic antennas, and material asymmetry in general, may offer many new routes toward novel nanophotonic sensing schemes.

19.
Nat Commun ; 2: 481, 2011 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-21934665

RESUMO

Recent progress in nanophotonics includes demonstrations of meta-materials displaying negative refraction at optical frequencies, directional single photon sources, plasmonic analogies of electromagnetically induced transparency and spectacular Fano resonances. The physics behind these intriguing effects is to a large extent governed by the same single parameter-optical phase. Here we describe a nanophotonic structure built from pairs of closely spaced gold and silver disks that show phase accumulation through material-dependent plasmon resonances. The bimetallic dimers show exotic optical properties, in particular scattering of red and blue light in opposite directions, in spite of being as compact as ∼λ(3)/100. These spectral and spatial photon-sorting nanodevices can be fabricated on a wafer scale and offer a versatile platform for manipulating optical response through polarization, choice of materials and geometrical parameters, thereby opening possibilities for a wide range of practical applications.

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